The sluggish reaction kinetics at the cathode/electrolyte interface of lithium–sulfur (Li–S) batteries limits their commercialization. Herein, we show that a dual-regulation system of iron phthalocyanine (FePc) and octafluoronaphthalene (OFN) decorated on graphene (Gh), denoted as Gh/FePc+OFN, accelerates the interfacial reaction kinetics of lithium polysulfides (LiPSs). Multiple in situ spectroscopy techniques and ex situ X-ray photoelectron spectroscopy combined with density functional theory calculations demonstrate that FePc acts as an efficient anchor and scissor for the LiPSs through Fe···S coordination, mainly facilitating their liquid–liquid transformation, whereas OFN enables Li-bond interaction with the LiPSs, accelerating the kinetics of the liquid–solid nucleation and growth of Li2S. This dual-regulation system promotes the smooth conversion reaction of sulfur, thereby improving the battery performance. A Gh/FePc+OFN-based Li–S cathode delivered an ultrahigh initial capacity of 1604 mAh g–1 at 0.2 C, with an ultralow capacity decay rate of 0.055% per cycle at 1 C over 1000 cycles.

Lithium–sulfur batteries suffer from poor cycling stability at high areal sulfur loadings (ASLs) mainly because of the infamous shuttle problem and the increasing diffusion distance for ions to diffuse along the vertical direction of the cathode plane. Here, a carbon nanotube (CNT)/graphene (Gra)‐S‐Al3Ni2 cathode with 3D network structure is designed and prepared. The 3D network configuration and the Al in the Al3Ni2 provide an efficient channel for fast electron and ion transfer in the three dimensions, especially along the vertical direction of the cathode. The introduction of Ni in the Al3Ni2 is able to suppress the shuttle effect via accelerating reaction kinetics of lithium polysulfide species conversion reactions. The CNT/Gra‐S‐Al3Ni2 cathode exhibits ultrahigh cycle‐ability at 1 C over 800 cycles, with a capacity degradation rate of 0.055% per cycle. Additionally, having high ASLs of 3.3 mg cm−2, the electrode delivers a high reversible areal capacity of 2.05 mA h cm−2 (622 mA h g−1) over 200 cycles at a higher current density of 2.76 mA cm−2 with high capacity retention of 85.9%. The outstanding discharge performance indicates that the design offers a promising avenue to develop long‐life cycle and high‐sulfur‐loading Li–S batteries.

Flexible lithium-ion batteries (FLBs) are of critical importance to the seamless power supply of flexible and wearable electronic devices. However, the simultaneous acquirements of mechanical deformability and high energy density remain a major challenge for FLBs. Through billions of years of evolutions, many plants and animals have developed unique compositional and structural characteristics, which enable them to have both high mechanical deformability and robustness to cope with the complex and stressful environment. Inspired by nature, many new materials and designs emerge recently to achieve mechanically flexible and high storage capacity of lithiumion batteries at the same time. Here, we summarize these novel FLBs inspired by natural and biological materials and designs. We first give a brief introduction to the fundamentals and challenges of FLBs. Then, we highlight the latest achievements based on nature inspiration, including fiber-shaped FLBs, origami and kirigami-derived FLBs, and the nature-inspired structural designs in FLBs. Finally, we discuss the current status, remaining challenges, and future opportunities for the development of FLBs. This concise yet focused review highlights current inspirations in FLBs and wishes to broaden our view of FLB materials and designs, which can be directly "borrowed" from nature.

Rechargeable aqueous zinc-ion batteries (AZIBs) have attracted more attention in large-scale energy storage systems arising from their unique merits, such as intrinsic safety, low cost, and relatively high theoretical energy...

The complicated reactions at the cathode–electrolyte interface in Li–S batteries are a large barrier for their successful commercialization. Herein, we developed a molecular design strategy and employed three small molecules acting as interfacial mediators to the cathodes of Li–S batteries. The theoretical calculation results show that the incorporation of tris­(4-fluorophenyl)­phosphine (TFPP) has a strong binding performance. The experimental results demonstrate that the strong chemical interactions between polysulfides and the F, P atoms in TFPP not only modify the kinetics of the electrochemical processes in the electrolyte but also promote the formation of short-chain clusters (Li2S x , x = 1, 2, 3, and 4) at the interface during the charge–discharge process. As a result, an optimized electrode exhibits a low capacity decay rate of 0.042% per cycle when the current rate is increased to 5 C over 1000 cycles.